The proposed research will study the dynamics of water in nanoscopic environments and water-protein interactions in nanoscopic environments using ultrafast multidimensional infrared stimulated vibrational echoes with full phase information. Such experiments provide vibrational echo correlation spectra, which are akin to multidimensional NMR techniques except that vibrational echo correlation spectroscopy directly examines the structural degrees of freedom of biological systems on time scales not accessible by other methods. The experiments and associated theory examine dynamics, structure and their interrelationship. The new work builds on the successful application of multidimensional vibrational echo methods by the Fayer research group. For decades, vibrational spectroscopy has been important in the study of biological systems. The application and development of vibrational echo correlation spectroscopy will enhance vibrational spectroscopy as a tool with an impact as great as the advance of magnetic resonance into multidimensional techniques.